I find Grima very disturbing. I noticed the tear too ... and although I feel he felt some regret, I think he was scared of the entire situation and what was happening. I believe at that moment he realized the seriousness of the situation & in some way wished he hadn't been a puppet of Saruman's. I pity him to some extent, and believe he had some kind of twisted love for Eowyn, but he didn't have to allow Saruman to get that kind of hold on him. Yes, Saruman is very persuasive & intimidating, and maybe Grima felt he had no choice. But he did have a choice ... and it was his own lack of courage that made him fall under Saruman's "spell."
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"....though in all lands love is now mingled with grief, it grows perhaps the greater." ~~ Haldir
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